Structure‐Guided Balancing of Ambipolar Transport Enables Symmetric Switching in Heterojunction Bilayer Organic Transistor Inverters

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ABSTRACT High inverter performance in ambipolar organic electronics requires balanced channel strengths rather than maximized single‐carrier mobility. Here, we demonstrate symmetric switching through balanced ambipolar transport in vertically stacked pentacene/ N , N ′‐ditridecylperylene‐3,4,9,10‐tetracarboxylic diimide (PTCDI‐C 13 ) heterojunction bilayers (HJBs) fabricated on polymer‐grafted SiO 2 dielectrics. By systematically tuning the nominal equivalent (1–4 monolayers, ML s) and thermal reorganization of the PTCDI‐C 13 underlayer, a structural symmetry window is identified in which intermolecular self‐assembly stabilizes both carrier mobility and threshold‐voltage alignment. Under optimized conditions (3 ML , 150°C annealed), nearly identical hole and electron mobilities (∼1.0 cm 2 V − 1 s − 1 ) and convergent threshold voltages enable complementary‐like inverters exhibiting high voltage gain (>200) and large noise margins under ±80 V operation. At absolute supply voltage (| V DD |) = 80 V, the extracted low‐ and high‐state noise margins are approximately 29.9–33.9 V, corresponding to approximately 75–85% of | V DD |/2. Notably, imbalanced charge transport degrades switching symmetry despite improved unipolar mobility, revealing a non‐monotonic relationship between molecular ordering and circuit performance. These results establish interface‐mediated self‐assembly as a structure‐guided route for engineering transport symmetry in organic HJBs, while broader material generality and manufacturing scalability remain to be established.

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